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EELS and Xanes Analysis of Plutonium and Cerium Edges From Titanate Ceramics for Fissile Materials Disposal

Published online by Cambridge University Press:  02 July 2020

J.A. Fortner
Affiliation:
Argonne National Laboratory, Chemical Technology Division, Argonne, IL60439
E.C. Buck
Affiliation:
Argonne National Laboratory, Chemical Technology Division, Argonne, IL60439
A.J. Kropf
Affiliation:
Argonne National Laboratory, Chemical Technology Division, Argonne, IL60439
A.J. Bakel
Affiliation:
Argonne National Laboratory, Chemical Technology Division, Argonne, IL60439
M.C. Hash
Affiliation:
Argonne National Laboratory, Chemical Technology Division, Argonne, IL60439
S.B. Aase
Affiliation:
Argonne National Laboratory, Chemical Technology Division, Argonne, IL60439
D.B. Chamberlain
Affiliation:
Argonne National Laboratory, Chemical Technology Division, Argonne, IL60439
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We report x-ray absorption near edge structure (XANES) and extended x-ray fine structure analysis (EXAFS) spectra from the plutonium Llll and cerium Lm edges in prototype titanate ceramic hosts for disposal of surplus fissile materials. These spectra were obtained using the MRCAT beamline at the Advanced Photon Source (APS). The XANES and EXAFS results are compared with electron loss spectra (EELS) determination of oxidation state from the plutonium MlV,V and cerium MlV,V edges [1,2]. The titanate ceramics studied are based upon the hafniumpyrochlore and zirconolite mineral structures and will serve as an immobilization host, containing as much as 10 weight % fissile plutonium, and 20 weight % (natural or depleted) uranium. Similar formulations were composed using cerium as a “surrogate” element, replacing both plutonium and uranium in the ceramic matrix. We find the plutonium to be present almost entirely as Pu (IV), while the cerium is clearly in a mixed III-IV oxidation state in the surrogate ceramic.

Type
Future of Microscopy: Ceramics, Composites, and Cement
Copyright
Copyright © Microscopy Society of America

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References

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